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Elucidating the significance of copper and nitrate speciation in Cu-SSZ-13 for N2O formation during NH3-SCR

Negahdar, Leila, Omori, Naomi E., Quesne, Matthew G., Frogley, Mark D., Cacho-Nerin, Fernando, Jones, Wilm, Price, Stephen W. T., Catlow, C. Richard A. ORCID: https://orcid.org/0000-0002-1341-1541 and Beale, Andrew M. 2021. Elucidating the significance of copper and nitrate speciation in Cu-SSZ-13 for N2O formation during NH3-SCR. ACS Catalysis 11 (21) , 13091–13101. 10.1021/acscatal.1c03174

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Abstract

Unwanted N2O formation is a problem that has been noted in selective catalytic reduction (SCR) where copper zeolite catalysts are utilized. With its immense global warming potential and long-term stability, elevated atmospheric N2O has already been identified as a future challenge in the war on climate change. This paper explores the phenomenon of N2O formation during NH3-SCR over Cu-SSZ-13 catalysts, which are currently commercialized in automotive emissions control systems, and proposes a link between N2O production and the local copper environment found within the zeolite. To achieve this, a comparison is made between two Cu-SSZ-13 samples with different copper co-ordinations produced via different synthesis methods. A combination of synchrotron X-ray absorption near-edge spectroscopy, UV–vis, Raman, and density functional theory (DFT) is used to characterize the nature of copper species present within each sample. Synchrotron IR microspectroscopy is then used to compare their behavior during SCR under operando conditions and monitor the evolution of nitrate intermediates, which, along with further DFT, informs a mechanistic model for nitrate decomposition pathways. Increased N2O production is seen in the Cu-SSZ-13 sample postulated to contain a linear Cu species, providing an important correlation between the catalytic behavior of Cu-zeolites and the nature of their metal ion loading and speciation.

Item Type: Article
Date Type: Publication
Status: Published
Schools: Chemistry
Cardiff Catalysis Institute (CCI)
Publisher: American Chemical Society
ISSN: 2155-5435
Funders: UK Catalysis Hub Consortium funded by EPSRC (portfolio grants EP/K014706/1, EP/K014668/1, EP/ K014854/1, EP/K014714/1, and EP/I019693/1).
Date of First Compliant Deposit: 14 December 2021
Date of Acceptance: 13 October 2021
Last Modified: 10 Nov 2022 10:14
URI: https://orca.cardiff.ac.uk/id/eprint/146133

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